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Citation: Mengjie Liu, Mengting Peng, Baoxia Dong, Yunlei Teng, Ligang Feng, Qiang Xu. Explicating the Role of Metal Centers in Porphyrin-Based MOFs of PCN-222(M) for Electrochemical Reduction of CO2[J]. Chinese Journal of Structural Chemistry, ;2022, 41(7): 220704. doi: 10.14102/j.cnki.0254-5861.2022-0057 shu

Explicating the Role of Metal Centers in Porphyrin-Based MOFs of PCN-222(M) for Electrochemical Reduction of CO2

  • 1.

    School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, Jiangsu 225002, China

  • Corresponding author: Baoxia Dong, bxdong@yzu.edu.cn Qiang Xu, qxuchem@yzu.edu.cn
    • Mengjie Liu and Mengting Peng contributed equally to this work.
  • Received Date: 16 March 2022
    Accepted Date: 4 April 2022
    Available Online: 15 April 2022

Figures(7)

  • The porphyrin-based MOFs formed by combining Zr6 clusters and porphyrin carboxylic acids with clear M-N4 active centers show unique advantages in electrocatalytic reduction of CO2 (CO2RR). However, its conductivity is still the bottleneck that limits its catalytic activity due to the electrical insulation of the Zr cluster. Therefore, the porphyrin-based MOFs of PCN-222(M) (M = Mn, Co, Ni, Zn) with explicit M-N4 coordination were combined with the highly conductive material carbon nanotube (CNT) for discussing the influence of metal centers on the CO2RR performance based on theoretical calculations and experimental observations. The results show that the PCN-222(Mn)/CNT, PCN-222(Co)/CNT, and PCN-222(Zn)/CNT all exhibit high selectivity to CO (FECO > 80%) in the range of -0.60 to -0.70 V vs. RHE. The FECOmax of PCN-222(Mn)/CNT (-0.60 V vs. RHE), PCN-222(Co)/CNT (-0.65 V vs. RHE), and PCN-222(Zn)/CNT (-0.70 V vs. RHE) are 88.5%, 89.3% and 92.5%, respectively. The high catalytic activity of PCN-222(Mn)/CNT and PCN-222(Co)/CNT comes from the excellent electron mobility of their porphyrin rings and their low ΔG*COOH (0.87 and 0.58 eV). It reveals that the strength of backbonding π of the transition metal and its influence on the electron mobility in the porphyrin ring can affect its CO2RR activity.
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